Makhlooghiazad Faezeh, O'Dell Luke A, Porcarelli Luca, Forsyth Craig, Quazi Nurul, Asadi Mousa, Hutt Oliver, Mecerreyes David, Forsyth Maria, Pringle Jennifer M
Institute for Frontier Materials, Deakin University, ARC Centre of Excellence for Electromaterials Science, Waurn Ponds, Victoria, Australia.
Joxe Mari Korta Center, POLYMAT, University of the Basque Country, Donostia-San Sebastian, Spain.
Nat Mater. 2022 Feb;21(2):228-236. doi: 10.1038/s41563-021-01130-z. Epub 2021 Nov 18.
Zwitterionic materials can exhibit unique characteristics and are highly tunable by variation to the covalently bound cationic and anionic moieties. Despite the breadth of properties and potential uses reported to date, for electrolyte applications they have thus far primarily been used as additives or for making polymer gels. However, zwitterions offer intriguing promise as electrolyte matrix materials that are non-volatile and charged but non-migrating. Here we report a family of zwitterions that exhibit molecular disorder and plasticity, which allows their use as a solid-state conductive matrix. We have characterized the thermal, morphological and structural properties of these materials using techniques including differential scanning calorimetry, scanning electron microscopy, solid-state NMR and X-ray crystallography. We report the physical and transport properties of zwitterions combined with lithium salts and a lithium-functionalized polymer to form solid or high-salt-content liquid electrolytes. We demonstrate that the zwitterion-based electrolytes can allow high target ion transport and support stable lithium metal cell cycling. The ability to use disordered zwitterionic materials as electrolyte matrices for high target ion conduction, coupled with an extensive scope for varying the chemical and physical properties, has important implications for the future design of non-volatile materials that bridge the choice between traditional molecular and ionic solvent systems.
两性离子材料可展现出独特的特性,并且通过改变共价连接的阳离子和阴离子部分可实现高度可调。尽管迄今为止已报道了其广泛的性质和潜在用途,但在电解质应用中,它们目前主要用作添加剂或用于制备聚合物凝胶。然而,两性离子作为非挥发性、带电但不迁移的电解质基质材料具有诱人的前景。在此,我们报道了一类表现出分子无序和可塑性的两性离子,这使得它们能够用作固态导电基质。我们使用差示扫描量热法、扫描电子显微镜、固态核磁共振和X射线晶体学等技术对这些材料的热、形态和结构性质进行了表征。我们报道了两性离子与锂盐以及锂功能化聚合物结合形成固体或高盐含量液体电解质的物理和传输性质。我们证明,基于两性离子的电解质能够实现高目标离子传输,并支持稳定的锂金属电池循环。将无序的两性离子材料用作高目标离子传导的电解质基质的能力,以及改变化学和物理性质的广泛空间,对未来设计能够在传统分子和离子溶剂体系之间做出选择的非挥发性材料具有重要意义。